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11.
Nolan M. Gallagher Hong-Zhou Ye Shuting Feng Jeffrey Lopez Yun Guang Zhu Troy Van Voorhis Yang Shao-Horn Jeremiah A. Johnson 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(10):3980-3983
We present the discovery of a novel radical cation formed through one-electron oxidation of an N-heterocyclic carbene–carbodiimide (NHC–CDI) zwitterionic adduct. This compound possesses a distonic electronic structure (spatially separate spin and charge regions) and displays persistence under ambient conditions. We demonstrate its application in a redox-flow battery exhibiting minimal voltage hysteresis, a flat voltage plateau, high Coulombic efficiency, and no performance decay for at least 100 cycles. The chemical tunability of NHCs and CDIs suggests that this approach could provide a general entry to redox-active NHC–CDI adducts and their persistent radical ions for various applications. 相似文献
12.
Yuwei Gu Julia Zhao Jeremiah A. Johnson 《Angewandte Chemie (International ed. in English)》2020,59(13):5022-5049
Polymer networks, which are materials composed of many smaller components—referred to as “junctions” and “strands”—connected together via covalent or non‐covalent/supramolecular interactions, are arguably the most versatile, widely studied, broadly used, and important materials known. From the first commercial polymers through the plastics revolution of the 20th century to today, there are almost no aspects of modern life that are not impacted by polymer networks. Nevertheless, there are still many challenges that must be addressed to enable a complete understanding of these materials and facilitate their development for emerging applications ranging from sustainability and energy harvesting/storage to tissue engineering and additive manufacturing. Here, we provide a unifying overview of the fundamentals of polymer network synthesis, structure, and properties, tying together recent trends in the field that are not always associated with classical polymer networks, such as the advent of crystalline “framework” materials. We also highlight recent advances in using molecular design and control of topology to showcase how a deep understanding of structure–property relationships can lead to advanced networks with exceptional properties. 相似文献
13.
Nathan J. Oldenhuis K. Peter Qin Shu Wang Hong‐Zhou Ye Eric A. Alt Adam P. Willard Troy Van Voorhis Stephen L. Craig Jeremiah A. Johnson 《Angewandte Chemie (International ed. in English)》2020,59(7):2784-2792
Photoresponsive materials that change in response to light have been studied for a range of applications. These materials are often metastable during irradiation, returning to their pre‐irradiated state after removal of the light source. Herein, we report a polymer gel comprising poly(ethylene glycol) star polymers linked by Cu24L24 metal–organic cages/polyhedra (MOCs) with coumarin ligands. In the presence of UV light, a photosensitizer, and a hydrogen donor, this “polyMOC” material can be reversibly switched between CuII, CuI, and Cu0. The instability of the MOC junctions in the CuI and Cu0 states leads to network disassembly, forming CuI/Cu0 solutions, respectively, that are stable until re‐oxidation to CuII and supramolecular gelation. This reversible disassembly of the polyMOC network can occur in the presence of a fixed covalent second network generated in situ by copper‐catalyzed azide‐alkyne cycloaddition (CuAAC), providing interpenetrating supramolecular and covalent networks. 相似文献
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Junggi Ha Jeremiah D. Hogan David A. Laude 《Journal of the American Society for Mass Spectrometry》1993,4(2):159-167
The ionization of tetraphenylporphyrin (TPP) in a laser-desorbed metal ion plasma is examined by Fourier transform ion cyclotron resonance (FT-ICR) mass spectrometry. Competitive reaction pathways observed to generate abundant molecular ion species include electron detachment, cation attachment, charge exchange, metallation, and transmetallation in the positive ion mode and electron capture, metallation, and transmetallation in the negative ion mode. In general, cation attachment reactions dominate positive ion spectra below the laser irradiance threshold for plasma ignition, although the metallation product from [TPP]+ reaction with the metal atom, M, is observed. Negative ion products are not observed in the FT-ICR spectrum when a plasma is not formed. Under plasma ignition conditions, positive ion spectra include [TPP]+ formed by charge exchange with M+, which is also present in the spectrum. Negative ion spectra are dominated by [TPP]?; which is formed by attachment to thermal electrons generated in the plasma. Metallation reactions involving TPP and the metal substrate are examined. Positive ion metallation products are observed both in the absence of a plasma through reaction of [TPP]+ with M and by a second pathway under plasma ignition conditions through reaction of TPP with M+. In negative ion mode, metallation is only observed under plasma ignition conditions through reaction of [TPP]? with M. Observation of metallated products is found to be consistent with formation of stable metal oxidation states in the metallated porphyrin. 相似文献
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[reaction: see text] From a common precursor, two unusual dehydrobenzoannulene topologies have been synthesized utilizing either Pd-catalyzed or Cu-mediated oxidative homocoupling as the ring-closure step. 相似文献
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Jeremiah Rushchitsky 《Comptes Rendus Mecanique》2002,330(3):175-180
The problem of self-switching plane waves in elastic nonlinearly deformed materials is formulated. Reduced and evolution equations, which describe the interaction of two waves the power pumping wave and the faint signal wave are obtained. For the case of wave numbers matching the pumping and signal waves, a procedure of finding the exact solution of evolution equations is described. The solution is expressed by elliptic Jacobi functions. The existence of the power wave self-switching is shown and commented. To cite this article: J. Rushchitsky, C. R. Mecanique 330 (2002) 175–180. 相似文献
20.
Jeremiah G. Murphy 《Journal of Elasticity》2007,86(2):139-154
The form of the classical stress–strain relations of linear elasticity are considered here within the context of nonlinear
elasticity. For both Cauchy and symmetric Piola-Kirchhoff stresses, conditions are obtained for the associated strain fields
so that they are independent of the material constants and compatible with existence of a strain–energy function. These conditions
can be integrated in both cases to obtain the most general strain field that satisfies these conditions and the corresponding
strain–energy function is obtained. In both cases, a natural choice of form of solution is suggested by the special case of
the compatibility conditions being satisfied identically. It will be shown that some strain–energy functions previously introduced
in the literature are special cases of the results obtained here. Some recent linear stress–strain relations, proposed in
the context of Cauchy elasticity, are examined to see if they are compatible with hyperelasticity.
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